Energy- and carbon-efficient CO2/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption

Adnan Ozden, Jun Li (), Sharath Kandambeth, Xiao-Yan Li, Shijie Liu, Osama Shekhah, Pengfei Ou, Y. Zou Finfrock, Ya-Kun Wang, Tartela Alkayyali, F. Pelayo García de Arquer, Vinayak S. Kale, Prashant M. Bhatt, Alexander H. Ip, Mohamed Eddaoudi (), Edward H. Sargent () and David Sinton ()
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Adnan Ozden: University of Toronto
Jun Li: University of Toronto
Sharath Kandambeth: King Abdullah University of Science and Technology
Xiao-Yan Li: University of Toronto
Shijie Liu: University of Toronto
Osama Shekhah: King Abdullah University of Science and Technology
Pengfei Ou: University of Toronto
Y. Zou Finfrock: Argonne National Laboratory
Ya-Kun Wang: University of Toronto
Tartela Alkayyali: University of Toronto
F. Pelayo García de Arquer: The Barcelona Institute of Science and Technology
Vinayak S. Kale: King Abdullah University of Science and Technology
Prashant M. Bhatt: King Abdullah University of Science and Technology
Alexander H. Ip: University of Toronto
Mohamed Eddaoudi: King Abdullah University of Science and Technology
Edward H. Sargent: University of Toronto
David Sinton: University of Toronto

Nature Energy, 2023, vol. 8, issue 2, 179-190

Abstract: Abstract Carbon dioxide/monoxide (CO2/CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface—a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The π-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation–π interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. As a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm−2.

Date: 2023
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DOI: 10.1038/s41560-022-01188-2

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